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Abstract: The use of organic silane monomers in the preparation of substrate-selective polymers by molecular imprinting is described. Silanes are allowed to polymerize on the surface of porous silica particles in aqueous solution. The resulting polysiloxane copolymer becomes covalently anchored to silanol groups of the original silica. such preparations retain the rigidity of the silica matrix and can therefore be used in high-performance liquid chromatography. Polysiloxane copolymers imprinted with the dyes rhodanile blue or safranine O showed preferential binding of the respective compound. The observed recognition is believed to occur because cavities containing specific binding groups for the dyes at defined positions are developed during the polymerization procedure. In this context the synthesis of a new silane, boronatesilane, was carried out. This compound was included in the monomer mixture used for the preparation of a polysiloxane-coated silica showing affinity for the glycoprotein transferrin. Organic silanes were also used for entrapment of enzymes, resulting in block polymers, which after fragmentation yielded relatively high recoveries of enzyme activity. Alternatively, the entrapment/polymerization was allowed to proceed on the surface of porous silica, in analogy with the imprinting procedure, resulting in entrapped enzyme preparations with high mechanical stability.